The synthesis of arrays of aligned multi-wall carbon nanotubes (CNTs) by thermal chemical vapor deposition is addressed in this study. Deposition experiments are carried out in a hot-wall reactor from mixtures of acetylene and helium, using iron coated silicon wafers as substrates. Scanning electron microscopy (SEM) is employed to discuss the growth mechanisms and the interaction between the substrate and the aligned CNTs film. Methods for improved substrate-CNTs film interaction are proposed, aiming at fabricating a more efficiently controllable and scalable process, adjusted to meet the forthcoming industrial demands.